Abstract
In this paper, effects of the spatial nonuniformity of an optical near field (ONF) on the molecular photodissociation process are presented. The dissociation dynamics of ${{\mathrm{H}}_{2}}^{+}$ was theoretically investigated by solving a non-Born-Oppenheimer Schr\odinger equation. It was found that in addition to two dissociation mechanisms, which are one-photon and three-photon processes induced by uniform laser light excitation, the nonuniform ONF opens another dissociation path: two-step excitation mediated by vibrationally excited states. The nonuniformity of the ONF causes a transition between vibrational states that is forbidden according to conventional selection rules, leading to the dissociation path. The dependences of photodissociation on the intensity and nonuniformity of the ONF were calculated and the results validated the two-step dissociation mechanism.
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